The DOE is currently conducting cleanup activities at its nuclear weapons development sites, many of which have accumulated plutonium (Pu) in soils for 50 years. To properly control Pu migration within Federal areas and onto public lands, to better evaluate the public risk, and to design effective remediation strategies, a fundamental understanding of Pu speciation and environmental transport is needed. Our goal is to use characterization, mobility, thermodynamic, and mineral-interaction data to develop better models of radionuclide transport and risk assessment which will enable the development of science-based decontamination strategies. In addition, if direct characterization of Pu in samples from a contaminated site reveal that the Pu is predominantly in an exceedingly low soluble, low mobility form, then acceptable, reasonable limits for site remediation and closure can be set in a directly defensible manner. Our overarching research approach has the following three interrelated facets: characterization of Pu in samples from a contaminated site; fundamental study of environmentally-relevant Pu species; and thermodynamic geochemical modeling of PU speciation and mobility. This approach differs from those of most other projects funded at a similar level because of its very broad scope and the range of specific methods and techniques used in the research. While one can argue that our approach is overly ambitious, it is absolutely mandated by the state of actinide environmental science. Unlike most other contaminant metals, the knowledge on Pu within each of these subfields is woefully inadequate to support site remediation and stewardship.